臺灣博碩士論文加值系統

多環芳香烴碳氫化合物(PAHs)具疏水性，屬於致癌物質，大量工業廢水排放導致水中PAHs濃度上升，造成環境嚴重衝擊。因此如何將PAHs從水中移除已成非常重要的課題。 本研究利用共沉澱方法合成Mg2Al-(NO3-) LDH (2:1LDH)，再以離子交換方式將化學界面活性sodium dodecyl sulfate (SDS) 及生物界面活性劑 rhamnolipid (RL)修飾2:1LDH合成SDS-LDH及RL-LDH作為移除水中Naphthalene (NaP)、Acenaphthylene (AcPy)以及Acenaphthene (AcP)等三種PAHs之吸附劑。等溫吸附實驗結果顯示，相同重量的RL-LDH對於NaP的吸附能力較SDS-LDH高，主要是因為RL-LDH 層間間距較大，有機碳含量高，因此對於NaP有較多的分配位置，故對於水中NaP的移除效率較大。動力吸附實驗結果顯示，SDS-LDH以及RL-LDH移除水中NaP經反應15分鐘後即可達到平衡，並較適合以Elovich方程式來描述。溫度效應結果顯示，SDS-LDH以及RL-LDH對於NaP的移除量會隨著溫度增加而降低。當改變初始pH以及離子強度對於SDS-LDH以及RL-LDH對於NaP的移除量影響是較小的。PAHs間物種的影響結果顯示，RL-LDH對於疏水性較高的AcPy有較大的吸持含量，其次為AcP，最低者為NaP。回收再利用試驗結果得知，RL-LDH重複利用數可達五次以上，且仍有75 %的移除效率 。經由生物界面活性劑(RL)與化學界面活性劑(SDS)修飾後之LDH皆能對水中PAHs有良好的移除效果，並且以RL-LDH對於PAHs具有更大的移除效果。RL 相較於 SDS 毒性低，同時RL-LDH並具有可重複利用性，因此對水中PAHs的移除，RL-LDH是一種具有潛力及對環境友善的吸附劑。

Sorption is a common treatment for removing pollutants from natural environments. The sorption of polycyclic aromatic hydrocarbons (PAHs) by layered double hydroxide (LDHs) and surfactant modified LDHs had been investigated. Mg2-Al (NO3) LDH has been synthesized by co-precipitation method with interlayer nitrate and the Mg/Al molar ratio was 2. Chemical synthesis surfactant sodium dodecyl sulfate (SDS) and biosurfactant rhamnolipid (RL) modified LDHs, SDS-LDH and RL-LDH, were synthesized by ion exchange method. The experimental results indicated that more organic carbon content and larger interlayer spacing lead RL-LDH sorb more naphthalene (NaP) than SDS-LDH. The fitted sorption data revealed that the Elovich model could be best described the sorption kinetics, respectively. The temperature has significantly influenced sorption of NaP on SDS-LDH and RL-LDH : lower temperature leads to more sorption capacity. The sorption process was almost unaffected by NaP initial pH and ionic strength. Additionally, acenaphthene (AcP) and acenaphthylene (AcPy) could be sorbed more than NaP by RL-LDH cause of the higher octanol-water partition coefficient.The desorption and reuse experiments revealed that RL-LDH could be used more than 5 times and the removal efficiency is higher than 75% Consequently, RL-LDH has low toxicity and reuse ability make it be a potential adsorbent for organic pollutant removal from aqueous solution.

目 錄
口試委員審定書…………………………………………………………I
誌謝……………………………………………………………………...II
中文摘要………………………………………………………………..III
英文摘要………………………………………………………………...V
目錄……………………………………………………………………..VI圖目錄…………………………………………………………………..IX
表目錄………………………………………………………………….XII
第一章 前言…………………………………………………..…………1
第二章 文獻回顧…………………………...………………..……….…3
2-1多環芳香烴化合物的基本性質及危害……………………..………3
2-1-1 多環芳香烴化合物的基本性質………………………………….3
2-1-2多環芳香烴化合物之來源與在環境中的分佈………………..…7
2-1-3多環芳香烴化合物的危害………………………………………...8
2-2 層狀雙氫氧化物之來源與應用…………………………………….9
2-2-1層狀雙氫氧化物…………………………………….……………..9
2-3界面活性劑……………………………………….…………...……15
2-3-1 化學界面活性劑…………………………….……….….………15
2-3-2生物界面活性劑…………………………………….…………....19
2-3-3界面活性劑修飾層狀雙氫氧化物對於水中有機污染物的應用
……………………………………….………………………..…...25
第三章 材料與方法………………….………………………………...29
3-1實驗設計……………………………………………………………29
3-2層狀雙氫氧化物(LDH)之製備………………….…………………30
3-2-1合成Mg2-Al(NO3) LDH…………….………………....................30
3-2-2 製備SDS-LDH…………….……………….................................31
3-2-3 RL-LDH之條件選定及製備…………….………………............31
3-3層狀雙氫氧化物的基本性質…………….………………………...34
3-3-1化學組成分析…………….………………………........................34
3-3-2. X光繞射分析…………….……………………….......................35
3-3-3. 官能基之測定…………….……………………….....................35
3-3-4. 電子顯微鏡…………….……………………….........................36
3-4水中多環芳香烴化合物之配製及測定……………………………37
3-5吸附實驗…………….………………………….…………...……...41
3-5-1. 動力吸附…………….………………………….…………...….41
3-5-2. 等溫吸附…………….………………………….…………...….42
3-5-3. 溫度效應…………….………………………….…………...….42
3-5-4. pH值效應…………….………………………….…………...…43
3-5-5. 離子強度影響…………….………………………….…………43
3-5-6. 競爭效應…………….………………………….…………........44
3-6 脫附實驗及吸附劑回收再利用效益…………….………………..45
3-6-1. 脫附實驗…………….………………………….…………........45
3-6-2. 吸附劑回收再利用效益…………….………………………….45
第四章 結果與討論…………….………………………….…………46
4-1 吸附劑基本性質之探討…………….………………………….….46
4-2吸附實驗…………….………………………….…………...……...72
4-2-1 等溫吸附實驗…………….………………………….………….72
4-2-2 動力吸附實驗…………….………………………….…….........76
4-2-3 溫度效應…………….………………………….…….................80
4-2-4 初始pH效應…………….………………………….……………81
4-2-5 離子強度效應…………….………………………….………….84
4-2-6 PAHs物種間的影響…………….………………………….….....86
4-3 脫附及回收再利用試驗…………….………………………….….88
第五章 結論…………….………………………….…..........................90
第六章 參考文獻…………….………………………………………...92


圖目錄
圖一、美國環保署列為16 種優先處理之多環芳香烴化合物…………4
圖二、層狀雙氫氧化物之結構示意圖………….…………….………10
圖三、等溫吸附曲線之四種型態………….…………….……………..12
圖四、界面活性劑濃度對表面張力、界面張力及污染物溶解度影響之
概要圖………….…………….……………….…………….…..17
圖五、界面活性劑於臨界微胞濃度前後之結構示意圖.……………...17
圖六、生物界面活性劑rhamnolipid (R1及R2)之結構式及化學式…..22
圖七、Naphthalene之GC/FID分析圖譜………………….……………39
圖八、Acenaphthylene之GC/FID分析圖譜……….…………………...39
圖九、Acenaphthene之GC/FID分析圖譜…….………………………..40
圖十、NaP、AcPy及AcP濃度為2 mg L-1之GC/FID分析圖譜…….…40
圖十一、 Mg2-Al-(NO3) LDH (2:1LDH)之X-ray 繞射光譜圖…….…47
圖十二、LDH及CLDH對於rhamnolipid插層效應的影響….………..51
圖十三、rhamnolipid濃度對於插層效應的影響….………….………. 52
圖十四、不同溫度對於rhamnolipid插層效應的影響….………..……54
圖十五、不同固液比對於rhamnolipid插層效應的影響….…………...56
圖十六、不同反應時間對於rhamnolipid插層效應的影響….……….58
圖十七、2θ為3到50o時LDH、SDS-LDH及RL-LDH之X-ray繞射
光譜圖….……….……….………….……….………….…………60
圖十八、2θ為0.5到10o時LDH、SDS-LDH及RL-LDH之X-ray繞
射光譜圖……….………….………….………….………….…….61
圖十九、2:1LDH、SDS-LDH及RL-LDH之結構示意圖…….….….63
圖二十、2:1LDH、SDS-LDH及RL-LDH之SEM影像圖示…….……65
圖二十ㄧ、2:1LDH、SDS、SDS-LDH、RL及RL-LDH之FTIR光譜圖…….………….………….…….………….………….…………68
圖二十二、2:1LDH、SDS-LDH及RL-LDH對NaP之等溫吸附曲線………….………….………….………….………….…….……74
圖二十三、2:1LDH、SDS-LDH及RL-LDH對NaP之動力吸附曲線…77
圖二十四、2:1LDH、SDS-LDH及RL-LDH對於NaP(a)一級，(b)二級，(c)Elovich之線性迴歸動力吸附實驗…….………….………78
圖二十五、SDS-LDH及RL-LDH在不同溫度下對於NaP吸附結果...80
圖二十六、SDS-LDH及RL-LDH在不同溫度下對於NaP吸附結果...83
圖二十七、不同pH對於Mg3-Al(NO3) LDH及SDS-LDG中Mg 及 Al
溶解度之影響…….………….………….………….…………..83
圖二十八、RL-LDH對NaP再利用及脫附效率…….………………..85
圖二十九、AcP及AcPy對於RL-LDH吸持NaP之影響.……….………87
圖三十、RL-LDH對於NaP脫附試驗及回收再利用次數之吸附結果……….…………….…………….…………….…………….…89


表目錄
表一、16種PAHs之物化特性……….…………….…………….………5
表二、四種常見之陰離子型界面活性劑……….…………….………26
表三、不同條件下所製備而成之RL-LDH及其命名……….….……33
表四、Mg2-Al-(NO3) LDH之組成特性……….…………….…………48
表五、2:1 LDH, SDS-LDH 及 RL-LDH之FTIR圖譜資料…………..69
表六、LDH、SDS-LDH及RL-LDH之組成特性……….…………….71
表七、2:1LDH、SDS-LDH及RL-LDH之化學組成分析和結構式….71
表八、SDS-LDH及RL-LDH對NaP之等溫吸附實驗參數……….…75
表九、2:1LDH、SDS-LDH及RL-LDH對NaP之動力吸附參數………79

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